Efficient and Stable Inverted Perovskite Solar Modules Enabled by Solid–Liquid Two-Step Film Formation

Highlights High-quality large-area perovskite films are prepared using a solid–liquid two-step film formation method combined with CsBr modification for the buried interface and Urea additive for perovskite crystallization. The inverted perovskite solar modules’ performance is enhanced to 20.56% in 61.56 cm2 with improved stability. Supplementary Information The online version contains supplementary material available at 10.1007/s40820-024-01408-2.

insights into the charge carrier dynamics, which was fitted using an empirical biexponential equation: 48 y = A 1 exp ( -t τ 1 ) +A 2 exp ( -t τ 2 ) +y 0 The average PL lifetime is determined by the following equation: where y0 is the decay constant, A1 and A2 are decay amplitudes, τ1 is the fast decay process associated with the charge transfer, and τ2 is the slow decay process resulting from charge recombination.

In-situ photoluminescence measurements
In-situ photoluminescence (in-situ PL) spectra were characterized by home-built equipment, including an excitation system, fiber system, and detector system.The testing samples are held in a temperature-controlled N2 glove box or humidity-controlled air box with a fiber system set around the sample, while the excitation and detection system is set in the ambient environment connected with the fiber.An excitation system was used using an excitation laser (315 nm, max = 300 W).Excitation light was introduced to the sample through a fiber.The emitted light from the sample was collected by fiber and introduced to a spectrophotometer (Ocean Optics USB2000).A 550 nm low pass filter is applied in the light pass to the spectrophotometer.

Perovskite photovoltaic mini-modules fabrication and characterization.
For the large-size perovskite modules, laser etching, including P1, P2, and P3 processes, was conducted by a nanosecond laser (ZNLB-22V1-LW300).Before use, the FTO was cleaned with ultraviolet ozone for 15min.The following procedures were fabricated on the prepatterned large FTO glass substrates.The mini-modules were fabricated on the pre-patterned large FTO glass substrates (10×10 cm).For the P1 process,10 cm × 10 cm size FTO substrates were patterned with a scribing width of 35 μm with 11-strip connected in series.The NiOx films were prepared by magnetron sputtering at 9 ×10 -4 Pa, and the power was controlled at 500 W for 300s, and the thickness was about 25 nm.The first step for the PSM fabrication is different for the blade-coating and solid-liquid process.For the blade-coating process, the solution of PbI2 (461 mg) in 1mL DMF: DMSO (10:1) was blade-coated onto the above substrate at a movement speed of 20 mm s -1 in air.For the solid-liquid process, CsBr (15 nm) and PbI2 (300nm) were deposited sequentially by thermal evaporation on the NiOx substrates.For the second step, the solution of FAI: MACl (110 mg: 11 mg) in the absence or the presence of Urea in 1 mL IPA was blade-coated onto the above PbI2-covered FTO glass substrates at a movement speed of 15 mm s -1 in air.The N2 knife worked at 0.5 kaf cm -2 during blade-coating.Then, the film was annealed at 150 ℃ for 20 min in air with a relative humidity of 40 ± 5%.Afterward, 25 nm C60, 5 nm BCP, and 240 nm copper were sequentially deposited sequentially using thermal evaporation under a high vacuum (≤8 × 10 −4 Pa).For the P3 process, the Cu layer was scribed with a 95 µm width.A full structure of the large-size PSC is shown in Fig. S13.The fabricated modules typically have 11 sub-cells, each with a width of 7.33 mm.The total dead width was 0.332 mm, giving a GFF of 95.47%.
The mini-modules were fabricated on the pre-patterned large FTO glass substrates (10×10 cm, P1 width 35 μm) following the same procedure as the solar cells.The fabricated modules typically have 11 sub-cells, each with a width of 7.33 mm.The laser scribing was performed twice with a laser marker.The final widths of P2 and P3 were measured to be 116 and 95 μm, respectively.The total scribing line width was 0.332 mm, giving a GFF of 95.47%.
The current density-voltage (J-V) characteristics of the mini-modules were measured using a Keithley 2400 Source Meter under standard AM1.5 G illumination, and the light intensity was calibrated using a standard silicon reference cell (Newport, Oriel Sol3Atm).The J-V curves were measured by forward scan (-0.1 to 13 V) and reverse scan (13 to -0.1 V).EQE spectra were obtained with a PVE300-IVT QE measurement kit by focusing a monochromatic light beam onto the devices.
4. Supplementary Figures.Table S1.Photovoltaic parameters of PVSK based on solid-liquid with different deposition rates.

Fig. S2 .
Fig. S2.The SEM images of PbI2 prepared by vapor deposition with different rates.

Fig. S4 .
Fig. S4.The GIWAXS line-cut profiles of perovskite films (prepared by blade coating and

Fig. S6 .
Fig. S6.The SEM images and grain size distribution of PVSK/CsBr + Urea film with varying

Fig. S8 .
Fig. S8.(a) The UV-vis absorption spectrum of perovskite films and (b) the corresponding

Fig. S11 .
Fig. S11.The manufacturing procedure of perovskite film deposited by the solid-liquid two-

Fig. S12 .
Fig. S12.The photos and XRD patterns of nine-portion perovskite films prepared by (a, b)

Table S3 .
Photovoltaic performance parameters of perovskite solar modules include p-i-n and n-i-p-type devices.